Evaluating the Structural Basis for Polar Altermagnet Candidate Ca$_{3}$(Ru,Ti)$_{2}$O$_{7}$

Abstract

The interplay between polar and altermagnetic orders remains largely unexplored in the broader landscape of correlated electron systems. Ca$_{3}$Ru$_{2}$O$_{7}$ has been proposed by density functional theory (DFT) as a polar altermagnet, reliant on the transformation of experimentally reported $Bb2_{1}m$ phase to a lower symmetry $Pn2_{1}a$ structure. Here, we perform a targeted search for the $Pn2_{1}a$ phase using synchrotron X-ray diffraction on single crystals of Ca$_{3}$Ru$_{2}$O$_{7}$ and Ca$_{3}$(Ru$_{0.99}$Ti$_{0.01}$)$_{2}$O$_{7}$. No diffraction signature of the $Pn2_{1}a$ structure is detected down to 20 K within experimental limits of $\sim$60-200 fm atomic displacements, significantly smaller than the DFT prediction of $\sim$1 pm. Combined with recent nonlinear transport measurements, our structural study suggests Ca$_{3}$Ru$_{2}$O$_{7}$ as a unique system where strong electron correlations drive an electronic phase transition without any measurable lattice symmetry change. With Ti substitution exceeding $\sim$3%, a chemically tunable altermagnetic phase with $Bb2_{1}m$ structure emerges. The study highlights the importance of sub-picometer metrology towards de-convolving structural versus electronic origins of altermagnets.